Stimuli‐Directed Colorimetric Interconversion of Helical Polymers Accompanied by a Tunable Self‐Assembly Process

Abstract Interconversion between extended and bent structures at the pendant groups of a chiral polyene framework [poly(phenylacetylene) with (R)‐(2‐methoxy‐2‐phenylacetyl)glycine residues linked to 4‐vinylanilines] allows the reversible colorimetric transformation from stretched to compressed helical cis‐transoid polyenic structures through manipulation of the flexible spacer. This transformation generates either organogels (stretched helical form) or nanoparticles (compressed helical form) under the control of polar/low polar stimuli respectively and opens the way to the development of new sensors and stimuli‐sensitive materials based on these concepts.